Status of Fission Yield Measurements
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nij»wiiM>iT»i»n'i»wwr I '• • «• PORTIOHS OF THIS &EPOTT ARE till •{•1& * i STATUS OF FI5.SIOM YIELD MEASUREHEMTS - i William J. Maeck Exxon Nuclear Idaho Company, Inc.* Idaho National Engineering Laboratory P.O. Box 2300 Idaho Fails, Idaho 83401, USA NOTICE . vtrpiird at Mt t*W. nm my < at i!tt$lte<K of anunwi my I*gal ! •prfn-nu Urn in uu *nuld noi | in(iuif.f privately 'IUWII n Prepared For Third ASTM-EURATOM Symposium On Reactor Dosimetry To be held at Ispra, Italy October 1-5, 1979 rUnder U^S... Department of Energy Idaho Operations Office Contract £- /L- - AC 07- 7c!XV>o 1. INTRODUCTION Fission yield data, for all neutron energies, play an important role in f many of the disiplines (fuel burnup, /ission rate measurements, dosimetry, reactor physics, damage studies, post irradiation fuel analysis, etc-) being discussed at this symposium. This paper reviews and presents a brief discussion i of the current status of fission yield measurement programs being conducted in the major laboratories throughout the world, and when possible, to—identify future activities. The contents of this paper are based on tv/o sources: 1) a mailing by the author to various principal investigators furnishing a form which could be used to describe their most current work, and 2) reference to the most recent IAEA Nuclear Data Section document "Progress in Fission Product Nuclear Data" , which is a compilation of current measurement activities relative i to fission product nuclear data, • • , The~gGnera-l-orgunizat.ij?Jl_oI._t]ie,.p.aper_Js..by-_f.issioning. nud.ide-and-the 1 ' i RewtTOrr~Bnergy~reg"ton-being~examined. , • , /\ i? -•• r \ AC T / \ v • /• ;'•• i ; <££, Vi<>.,,-,. sj r .. 2. GENERAL REVIEW . , 1 i ' i 1 i 2.1 Fission Yield Measurements /• The principal laboratories currently engaged in more extensive fission yield measurements are located in France, Germany, India, Japan, Switzerland, United Kingdom, and USA. The most ambitious programs appear to be those being conducted in the USA. Perhaps the most extensive absolute yield measurement program, is the long- term program being conducted at the Idaho National Engineering Laboratory (INEL) by Maeck and co-workers-. In this program isotope dilution mass spectrometry, is used to measure thermal and fast reactor chain yields for over 40 stable and long-lived fission products. In the past few years absolute fission'yields have been reported for "JU, U, and J U fast fission , Pu and Pu fast fission3,240Pu and 242Pu fast fission4, 237Np fast fission5, and recently.235U and Pu thermal fission ' . In general, the uncertainties associated with the measured yields are in the ]-2% range, Currently,. y->eld-measu-»-ements-are-beihy- •/i-v 233 235 239 241 <-e«:,.t made-on samples of U, U, Pu, and Pu which -had-irradiated in a harder spectrum of Expweimenta.1 Breeder Reactor -II (EBR_lI), than those previously V,"V4,-!>' £\s:iv* yield , ^V;H^/»-- irra.j <>*-/<. ' /" reported. A new ixr-adia.tion-and measurement program for the Fast Flux Test i / ' Facility (FFTF) is discussed in-detoil in Section 4. <-^> " ! ' —p -• A companion effort ice lea ted-to the INEL program is the correlation of reactor'fission yields with neutron energy ' ,/ ' ! ' ' / ' ' ': Glendenin Gindler and co-workers of the* Argonne National Laboratory •(ANL) are currently conducting a systematic stud£ of fission yields versus1neutron ' energy for mono-energetic neutroris in the range of 0.1 to 8.0 HeV, using the ANL fast neutron generator. Thejmeasupement techniques are direct high resolution gamma ray spectrometry and radiochemi/cal separations. In general,'the uncertainties range fro-n 3-15%, depending on the/iiagnitude of the yield and the measurement ; • / • ; • ' : , v • , ' ; ? ^ p 1 (\ 1 1 technique. To date, mono-energetic yields have been published for JU ' and preliminary results have been reported for " Th . Similar experiments 233 235 239 '?"* i ' • are in progress for U, u, and Pu. - Nethaway and co-workers at the Lawrence Livermore Laboratory (Ll!±) have recently reported/^ Pu y4e-lds—for 14.8 MeV f-i-ss-ion and 4 "slightly degraded" fission spectrum , A t~tMs« program 75 fission products were measured in the 14.8 '' 'A ' MeV irradiation and 45 fission products in the critical assembly experiment. The measurement technique was direct high resolution gamma ray spectrometry. The average uncertainty associated with the reported yields is estimated'to be about 1 5% relative. Similar experiments have been completed for Am but no values have..yfil been reported,f©r~each~target-nuclide^,/a\ 1 imited number of independent and cumulative fractional yields are reported,/' • ' ' At Oak Ridge National Laboratory (ORNL) Dickans and co-workers hav3 recently •j 1 extracted fission yield data from an experiment designed to measure the total' beta and gamma energy release or a funtion of time for the short-term thermal fission of U, Pu, and Pu. Using a large volume Ge(Li) detector^, the yields for 16 and 36 mass chains were measured for 241 Pu and23 9Pu,thermal fission, respectively. The absolute uncertainties range from 3 to 25%, relative. The 211 • ' 15 239 1 Pu results have been published , and the Pu data are being prepared for publication. •' _ , _ . « ' •At. the Second ATSM-EURATOM Conference several laboratories associated with an interlaboratory reaction rate measurement program.uresented papers ' giving evaluated consensus fission yield data for those fission product isotopes of primary, interest to fission rate a(id dosimetry measurements. In this cooperative experiment, the measurement methoc was high resolution gamma spectrometry and the number of fissions was established using a fission chamber. It is ahticipated that a status report relative to this program will be presented in the current symposium. At tho Battelle Pacific Northwest Laboratories (PNL), Ballon and Reeder and 235 ' Co-workers have moasurod the independent and cumulative U thermal fission yields of some very neutron-rich nuclides usirig the "on-line" mass spectrometer SOLAR^Spectroineter for On-Line Analysis of RadionulcicJes) . This is'an on-line 235 • i mass spectrometer which incorporates a U target in a surface ionization source /A/,,,- •• ' located in the thermal column of a 1HW TRIGA reactor at Washington State University, Pullman, Washington, USA. In this instrument a short burst of neutrons from the TRIGA reactor is used to produce various isowers of Br, Rb, In, I,,and Co fission products within the surface ionization source. Selective: ionization performs the rapid chemical, separation to give the desiredinuclides AS beams of.iAns. The ions are collected on a moving tape collector system for a short time^interval during and after the neutron pulse. Beta arid gamma counting are used to follow the decay of the isomers to determine the yield of each. A knowledge of the particular decay schemes is the limiting factor associated with accuracy of the1results. •he ' ' More recent studies are directed on the characterization of individual delayed neutron emitters. Using a 1.5 Mw TRIGA reactor and the fission-fragment recoil mass spectrometer, 19 HIAWATHTHA , Wehring and co-workers at the University of Illinois, have measured 2Q-~21 ?35 ' '"'' ^> ' s^ and reported * ' U thermal fission yields^ «The technique is reported toproduce yields with associated uncertainties of M% relative for the largest'mass yields. A unique capability of this technique is that chain and independent yield data can be obtained for all nuclides vtflh' independent'yields greater than 0.1%. HIAWATHA, consisting of a cylindrical focusing; electrostatic analyzer and time-of-fl ight'/Mslstem, is used tp determine fragment masses v/hi 1 e fragment energy . i : v. • ; « • loss is used to identify fragment atomic numbers in' amult'iparameter' experiment. li ' , i All fragment velocities and charjge states are'covered in this direct1 physical I , i' /. • f measurement of fission yields. Mass resolution of d:.5 amu and atomic number •' ' resolution of about 1-Z has been achieved:'- Uncertainties- about--1%-have-bfen : , J -»ojp.:--' ' • •, • : • *€hievec)-.f.or-the-'Iaryest"Tirass yfeids- New work planned for this instrument is the / : ' -i • : • investigation of the dependence of prompt neutron yields on fission fragment mass, atomic number, and energy. • ' • ' At the Los Alamos Scientific Laboratory (LASL) recent efforts have centered #n ' ' ' -about the measurement of,the relative fission'yields of various krypton and xenon isotopes for thermal, degraded-fission-spectrum, and 14-MeV neutron-induced fission of 235U and 239Pu, and for degraded-fission-spectrum and 14-McV fission of 236U pro jip and IJ . Wolfsberg at LASL, in cooperation.with Meixier and Denschlag at the 43 ' ' ^ University of Maine, have recently reported fractional cumulative yields ofA U-<-'»Wd " -• 249 krypton and xenon isotopes' for the thermal fission of Cf and spontaneous fission of 250Cf. ' •' •" ! IV, • • , 7VI the United Kingdom the principal centers for fission yield measurements are at Dounrcay and Harwell. The Ooureay program, under the direction of W. Davis and V. M. Sinclair, is primarily directed to the measurement of the fast reactor yields of the stable isotopes of neodymiur.i and of S,1?, ' Cp,"* and Ce; isotopes of interest in tiie measurement of nuclear fuel burnup,. In this program samples of enriched U, l5U, Pu, and Pu are being irradiated in the Prototype Fast Reactor (PFR) at Dounreay. tt*«>s-expec-ted..th3t £he irradiation will be completed 235 239 241 by the end of 1979. For U, Pu, and PuJthe atom percent fission is expected to exceed 15%, and for cPu and ' Pu, 1 to 4A. The principal measurement technique will be isotope dilution mass spectrometry. The number of, fission will be determined using the heavy element difference method. Expected uncertainties are 2% relative for the fission yields for235 U and 239Pu and %6% for 238U, 240Ru, and ?41 * ' 22' Pu.